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Combination of binary active sites into heterogeneous porous polymer catalysts for efficient transformation of CO2 under mild conditions
Chinese Journal of Catalysis ( IF 16.5 ) Pub Date : 2021-04-01 , DOI: 10.1016/s1872-2067(20)63679-8
Zhifeng Dai , Yongquan Tang , Fei Zhang , Yubing Xiong , Sai Wang , Qi Sun , Liang Wang , Xiangju Meng , Leihong Zhao , Feng-Shou Xiao

Abstract The transformation of CO2 into cyclic carbonates via atom-economical cycloadditions with epoxides has recently attracted tremendous attention. On one hand, though many heterogeneous catalysts have been developed for this reaction, they typically suffer from disadvantages such as the need for severe reaction conditions, catalyst loss, and large amounts of soluble co-catalysts. On the other hand, the development of heterogeneous catalysts featuring multiple and cooperative active sites, remains challenging and desirable. In this study, we prepared a series of porous organic catalysts (POP-PBnCl-TPPMg-x) via the copolymerization metal-porphyrin compounds and phosphonium salt monomers in various ratios. The resulting materials contain both Lewis-acidic and Lewis-basic active sites. The molecular-level combination of these sites in the same polymer allows these active sites to work synergistically, giving rise to excellent performance in the cycloaddition reaction of CO2 with epoxides, under mild conditions (40 °C and 1 atm CO2) in the absence of soluble co-catalysts. POP-PBnCl-TPPMg-12 can also efficiently fixate CO2 under low-CO2-concentration (15% v/v N2) conditions representative of typical CO2 compositions in industrial exhaust gases. More importantly, this catalyst shows excellent recyclability and can easily be separated and reused at least five times while maintaining its activity. In view of their heterogeneous nature and excellent catalytic performance, the obtained catalysts are promising candidates for the transformation of industrially generated CO2 into high value-added chemicals.

中文翻译:

将二元活性位点组合成多相多孔聚合物催化剂,在温和条件下有效转化 CO2

摘要 通过与环氧化物的原子经济环加成将 CO2 转化为环状碳酸酯最近引起了极大的关注。一方面,尽管已经为该反应开发了许多非均相催化剂,但它们通常存在诸如需要苛刻的反应条件、催化剂损失和大量可溶性助催化剂等缺点。另一方面,具有多个协同活性位点的多相催化剂的开发仍然具有挑战性和可取性。在本研究中,我们通过金属卟啉化合物和不同比例的鏻盐单体共聚制备了一系列多孔有机催化剂(POP-PBnCl-TPPMg-x)。所得材料包含路易斯酸性和路易斯碱性活性位点。这些位点在同一聚合物中的分子水平组合允许这些活性位点协同工作,在温和条件(40 °C 和 1 atm CO2)下,在没有二氧化碳的情况下,在 CO2 与环氧化物的环加成反应中产生优异的性能。可溶性助催化剂。POP-PBnCl-TPPMg-12 还可以在代表工业废气中典型 CO2 成分的低 CO2 浓度(15% v/v N2)条件下有效固定 CO2。更重要的是,这种催化剂表现出优异的可回收性,可以轻松分离和重复使用至少五次,同时保持其活性。鉴于其多相性质和优异的催化性能,所获得的催化剂是将工业产生的 CO2 转化为高附加值化学品的有希望的候选者。
更新日期:2021-04-01
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